Densified HKUST-1 Monoliths as a Route to High Volumetric and Gravimetric Hydrogen Storage Capacity
David G. Madden, Daniel O’Nolan, Nakul Rampal, Robin Babu, Ceren Çamur, Ali Nabeeh Shakhs, Shi‐Yuan Zhang, Graham A. Rance, Javier Pérez, Nicola Casati, Carlos Cuadrado‐Collados, Denis O’Sullivan, Nicholas Rice, Thomas Gennett, Philip A. Parilla, Sarah Shulda, Katherine E. Hurst, Vitalie Stavila, Mark D. Allendorf, Joaquín Silvestre‐Albero, Alexander C. Forse, Neil R. Champness, Karena W. Chapman, David Fairen‐Jiménez
Abstract
We are currently witnessing the dawn of hydrogen (H 2 ) economy, where H 2 will soon become a primary fuel for heating, transportation, and longdistance and long-term energy storage. Among diverse possibilities, H 2 can be stored as a pressurized gas, a cryogenic liquid, or a solid fuel via adsorption onto porous materials. Metal-organic frameworks (MOFs) have emerged as adsorbent materials with the highest theoretical H 2 storage densities on both a volumetric and gravimetric basis. However, a critical bottleneck for the use of H 2 as a transportation fuel has been the lack of densification methods capable of shaping MOFs into practical formulations while maintaining their adsorptive performance. Here, we report a high-throughput screening and deep analysis of a database of MOFs to find optimal materials, followed by the synthesis, characterization, and performance evaluation of an optimal monolithic MOF ( mono MOF) for H 2 storage. After densification, this mono MOF stores 46 g L -1 H 2 at 50 bar and 77 K and delivers 41 and 42 g L -1 H 2 at operating pressures of 25 and 50 bar, respectively, when deployed in a combined temperaturepressure (25-50 bar/77 K 5 bar/160 K) swing gas delivery system. This performance represents up to an 80% reduction in the operating pressure requirements for delivering H 2 gas when compared with benchmark materials and an 83% reduction compared to compressed H 2 gas. Our findings represent a substantial step forward in the application of high-density materials for volumetric H 2 storage applications.